Graphene is an allotrophic form of carbon that consists of a two-dimensional hexagonal arrangement of carbon atoms. Each layer of graphene is essentially a one-atom-thick planar layer of carbon atoms that are bonded in a honeycomb crystal lattice. Graphene can be in forms having one, two, hundreds or thousands of graphene layers. The electrical, mechanical, optical and chemical properties of graphene make it attractive for applications in high performance electronic and optical devices and is expected to play a significant role in future technologies that span a range from consumer electronics, to devices for the conversion and storage of energy, to conformable biomedical devices for healthcare. To realize these applications, however, a low-cost method of synthesizing large areas of high-quality graphene is required. Current methods for growing high-quality large-area single-layer graphene that are compatible with roll-to-roll manufacturing are highly wasteful, destroying approximately 300 kg of copper foil (thickness=25 μm) for every 1 g of graphene produced. Efforts to reduce this waste have been driven by two goals. The first goal is to reduce the cost and environmental impact for relatively high-end applications, i.e., nanoelectronics and transparent electrodes, for which graphene is currently regarded as an important component. The second goal is to enable potential applications, i.e., disposable electronics, textiles, conformable biomedical devices, and thin-film photovoltaic modules that would be difficult to realize using graphene at its current cost. In the well-known, roll-to-roll-compatible process originally described by Bae et al., (Bae, S., et. al., S. Nat. Nanotechnol. 2010, 5, 574.) single-layer graphene was grown on large-area copper foils by chemical vapor deposition (CVD) and released onto a carrier substrate by chemical etching of the copper. This process is significant in its ability to produce films over large areas, but the cost of a one-atom-thick layer of graphene includes the destruction of an equal area of a seventy thousand-atom-thick copper foil, along with the economic costs and environmental externalities associated with handling large amounts of corrosive waste. Thus, there is a need for improved methods of synthesizing large areas of high-quality graphene.